Near-Zero Emissions Oxy-Combustion Flue Gas Purification Task 3: SOx/NOx/Hg Removal for Low Sulfur Coal

The goal of this project was to develop a near-zero emissions flue gas purification technology for existing PC (pulverized coal) power plants that are retrofitted with oxycombustion technology. The objective of Task 3 of this project was to evaluate an alternative method of SOx, NOx and Hg removal from flue gas produced by burning low sulfur coal in oxy-combustion power plants. The goal of the program was to conduct an experimental investigation and to develop a novel process for simultaneously removal of SOx and NOx from power plants that would operate on low sulfur coal without the need for wet-FGD & SCRs. A novel purification process operating at high pressures and ambient temperatures was developed. Activated carbon's catalytic and adsorbent capabilities are used to oxidize the sulfur and nitrous oxides to SO{sub 3} and NO{sub 2} species, which are adsorbed on the activated carbon and removed from the gas phase. Activated carbon is regenerated by water wash followed by drying. The development effort commenced with the screening of commercially available activated carbon materials for their capability to remove SO{sub 2}. A bench-unit operating in batch mode was constructed to conduct an experimental investigation of simultaneous SOx and NOx removal from a simulated oxyfuel flue gas mixture. Optimal operating conditions and the capacity of the activated carbon to remove the contaminants were identified. The process was able to achieve simultaneous SOx and NOx removal in a single step. The removal efficiencies were >99.9% for SOx and >98% for NOx. In the longevity tests performed on a batch unit, the retention capacity could be maintained at high level over 20 cycles. This process was able to effectively remove up to 4000 ppm SOx from the simulated feeds corresponding to oxyfuel flue gas from high sulfur coal plants. A dual bed continuous unit with five times the capacity of the batch unit was constructed to test continuous operation and longevity. Full-automation was implemented to enable continuous operation (24/7) with minimum operator supervision. Continuous run was carried out for 40 days. Very high SOx (>99.9%) and NOx (98%) removal efficiencies were also achieved in a continuous unit. However, the retention capacity of carbon beds for SOx and NOx was decreased from ~20 hours to ~10 hours over a 40 day period of operation, which was in contrast to the results obtained in a batch unit. These contradictory results indicate the need for optimization of adsorption-regeneration cycle to maintain long term activity of activated carbon material at a higher level and thus minimize the capital cost of the system. In summary, the activated carbon process exceeded performance targets for SOx and NOx removal efficiencies and it was found to be suitable for power plants burning both low and high sulfur coals. More efforts are needed to optimize the system performance.